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1.
Angew Chem Int Ed Engl ; : e202404861, 2024 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-38738502

RESUMO

Solid oxide electrolysis cells are prospective approaches for CO2 utilization but face significant challenges due to the sluggish reaction kinetics and poor stability of the fuel electrodes. Herein, we strategically addressed the long-standing trade-off phenomenon between enhanced exsolution and improved structural stability via topotactic ion exchange. The surface dynamic reconstruction of the MnOx/La0.7Sr0.3Cr0.9Ir0.1O3-δ (LSCIr) catalyst was visualized at the atomic scale. Compared with the Ir@LSCIr interface, the in situ self-assembled Ir@MnOx/LSCIr interface exhibited greater CO2 activation and easily removable carbonate intermediates, thus reached a 42% improvement in CO2 electrolysis performance at 1.6 V. Furthermore, an improved CO2 electrolysis stability was achieved due to the uniformly wrapped MnOx shell of the Ir@MnOx/LSCIr cathode. Our approach enables a detailed understanding of the dynamic microstructure evolution at active interfaces and provides a roadmap for the rational design and evaluation of efficient metal/oxide catalysts for CO2 electrolysis.

2.
Angew Chem Int Ed Engl ; 63(5): e202313361, 2024 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-38088045

RESUMO

Cathodic CO2 adsorption and activation is essential for high-temperature CO2 electrolysis in solid oxide electrolysis cells (SOECs). However, the component of oxygen ionic conductor in the cathode displays limited electrocatalytic activity. Herein, stable single Ruthenium (Ru) atoms are anchored on the surface of oxygen ionic conductor (Ce0.8 Sm0.2 O2-δ , SDC) via the strong covalent metal-support interaction, which evidently modifies the electronic structure of SDC surface for favorable oxygen vacancy formation and enhanced CO2 adsorption and activation, finally evoking the electrocatalytic activity of SDC for high-temperature CO2 electrolysis. Experimentally, SOEC with the Ru1 /SDC-La0.6 Sr0.4 Co0.2 Fe0.8 O3-δ cathode exhibits a current density as high as 2.39 A cm-2 at 1.6 V and 800 °C. This work expands the application of single atom catalyst to the high-temperature electrocatalytic reaction in SOEC and provides an efficient strategy to tailor the electronic structure and electrocatalytic activity of SOEC cathode at the atomic scale.

3.
Natl Sci Rev ; 10(9): nwad078, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37565207

RESUMO

Solid oxide electrolysis cells provide a practical solution for the direct conversion of CO2 to other chemicals (i.e. CO), however, an in-depth mechanistic understanding of the dynamic reconstruction of active sites for perovskite cathodes during CO2 electrolysis remains a great challenge. Herein, we identify that iridium-doped Sr2Fe1.45Ir0.05Mo0.5O6-δ (SFIrM) perovskite displays a dynamic electrochemical reconstruction feature during CO2 electrolysis with abundant exsolution of highly dispersed IrFe alloy nanoparticles on the SFIrM surface. The in situ reconstructed IrFe@SFIrM interfaces deliver a current density of 1.46 A cm-2 while maintaining over 99% CO Faradaic efficiency, representing a 25.8% improvement compared with the Sr2Fe1.5Mo0.5O6-δ counterpart. In situ electrochemical spectroscopy measurements and density functional theory calculations suggest that the improved CO2 electrolysis activity originates from the facilitated formation of carbonate intermediates at the IrFe@SFIrM interfaces. Our work may open the possibility of using an in situ electrochemical poling method for CO2 electrolysis in practice.

4.
Angew Chem Int Ed Engl ; 62(32): e202307057, 2023 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-37285520

RESUMO

Perovskites exhibit excellent high-temperature oxygen evolution reaction (OER) activities as the anodes of solid oxide electrolysis cells (SOECs). However, the relationship between ion ordering and OER performances is rarely investigated. Herein, a series of PrBaCo2-x Fex O5+δ perovskites with tailored ion orderings are constructed. Physicochemical characterizations and density functional theory calculations confirm that the oxygen bulk migration and surface transport capacities as well as the OER activities are promoted by the A-site cation ordering, but weakened by the oxygen vacancy ordering. Hence, SOEC with the A-site-ordered and oxygen-vacancy-disordered PrBaCo2 O5+δ anode exhibits the highest performance of 3.40 A cm-2 at 800 °C and 2.0 V. This work sheds light on the critical role of ion orderings in the high-temperature OER performance and paves a new way for screening novel anode materials of SOECs.

5.
Front Immunol ; 13: 1018567, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36341405

RESUMO

Recurrent aphthous ulcer (RAU), one of the most common diseases in humans, has an unknown etiology and is difficult to treat. Thalidomide is an important immunomodulatory and antitumor drug and its effects on the gut microbiota still remain unclear. We conducted a metagenomic sequencing study of fecal samples from a cohort of individuals with RAU, performed biochemical assays of cytokines, immunoglobulins and antimicrobial peptides in serum and saliva, and investigated the regulation effects of thalidomide administration and withdrawal. Meanwhile we constructed the corresponding prediction models. Our metagenome-wide association results indicated that gut dysbacteriosis, microbial dysfunction and immune imbalance occurred in RAU patients. Thalidomide regulated gut dysbacteriosis in a species-specific manner and had different sustainable effects on various probiotics and pathogens. A previously unknown association between gut microbiota alterations and RAU was found, and the specific roles of thalidomide in modulating the gut microbiota and immunity were determined, suggesting that RAU may be affected by targeting gut dysbacteriosis and modifying immune imbalance. In-depth insights into sophisticated networks consisting of the gut microbiota and host cells may lead to the development of emerging treatments, including prebiotics, probiotics, synbiotics, and postbiotics.


Assuntos
Microbioma Gastrointestinal , Estomatite Aftosa , Humanos , Talidomida/uso terapêutico , Disbiose/complicações , Metagenoma
6.
Artigo em Chinês | WPRIM (Pacífico Ocidental) | ID: wpr-907002

RESUMO

Objective@# To investigate the classification of atrophic glossitis and to study the correlation between the classification and changes of VitB12, folic acid (FOL) and blood cell parameters@*Methods@#A total of 70 patients with atrophic glossitis (AG) were divided into complex type and simple type according to whether they had ulcer or erosion on the tongue mucosa or not. Another 65 healthy subjects during the same period were collected as the control group. The levels of vitamin B12, FOL and blood cell parameters were statistically analyzed using SPSS 25.0 software package.@*Results@#The levels of vitamin B12, red blood cell count (RBC) (3.52 ± 0.69) × 1012·L-1, hemoglobin (HGB)(11.97 ± 1.70) g·dL-1, white blood cell count (WBC) (4.85 ± 1.16) × 109·L-1, neutrophil count (NEUT) (2.76 ± 0.99) × 109·L-1, lymphocyte count (LYMPH) (1.48 ± 0.44) × 109·L-1 in complex type AG group were lower than those in simple type AG group (P<0.05). The levels of mean red blood cell volume (MCV) (104.90 ± 11.13) fL, mean corpuscular hemoglobin (MCH) (34.83 ± 4.56) pg, mean corpuscular hemoglobin concentration (MCHC) (331.09 ± 13.60) g·L-1 were higher than those in the simple type AG group (P<0.05). There was no significant difference in FOL content between these two groups (P>0.05). The levels of VitB12, MCV, MCH, MCHC, WBC, lymph and neut were correlated with the classification of atrophic glossitis (P < 0.05). @*Conclusion@#VitB12 deficiency was more apparent in complex AG, especially in large cell anemia, which correlated with the levels of WBC, NEUT, and LYMPH.

7.
Nat Commun ; 12(1): 5665, 2021 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-34580312

RESUMO

Metal nanoparticles anchored on perovskite through in situ exsolution under reducing atmosphere provide catalytically active metal/oxide interfaces for CO2 electrolysis in solid oxide electrolysis cell. However, there are critical challenges to obtain abundant metal/oxide interfaces due to the sluggish diffusion process of dopant cations inside the bulk perovskite. Herein, we propose a strategy to promote exsolution of RuFe alloy nanoparticles on Sr2Fe1.4Ru0.1Mo0.5O6-δ perovskite by enriching the active Ru underneath the perovskite surface via repeated redox manipulations. In situ scanning transmission electron microscopy demonstrates the dynamic structure evolution of Sr2Fe1.4Ru0.1Mo0.5O6-δ perovskite under reducing and oxidizing atmosphere, as well as the facilitated CO2 adsorption at RuFe@Sr2Fe1.4Ru0.1Mo0.5O6-δ interfaces. Solid oxide electrolysis cell with RuFe@Sr2Fe1.4Ru0.1Mo0.5O6-δ interfaces shows over 74.6% enhancement in current density of CO2 electrolysis compared to that with Sr2Fe1.4Ru0.1Mo0.5O6-δ counterpart as well as impressive stability for 1000 h at 1.2 V and 800 °C.

8.
Sensors (Basel) ; 20(15)2020 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-32707801

RESUMO

The SKA (Square Kilometer Array) radio telescope will become the most sensitive telescope by correlating a huge number of antenna nodes to form a vast array of sensors in a region over one hundred kilometers. Faceting, the wide-field imaging algorithm, is a novel approach towards solving image construction from sensing data where earth surface curves cannot be ignored. However, the traditional processor of cloud computing, even if the most sophisticated supercomputer is used, cannot meet the extremely high computation performance requirement. In this paper, we propose the design and implementation of high-efficiency FPGA (Field Programmable Gate Array) -based hardware acceleration of the key algorithm, faceting in SKA by focusing on phase rotation and gridding, which are the most time-consuming phases in the faceting algorithm. Through the analysis of algorithm behavior and bottleneck, we design and optimize the memory architecture and computing logic of the FPGA-based accelerator. The simulation and tests on FPGA are done to confirm the acceleration result of our design and it is shown that the acceleration performance we achieved on phase rotation is 20× the result of the previous work. We then further designed and optimized an efficient microstructure of loop unrolling and pipeline for the gridding accelerator, and the designed system simulation was done to confirm the performance of our structure. The result shows that the acceleration ratio is 5.48 compared to the result tested on software in gridding parts. Hence, our approach enables efficient acceleration of the faceting algorithm on FPGAs with high performance to meet the computational constraints of SKA as a representative vast sensor array.

9.
Angew Chem Int Ed Engl ; 59(37): 15968-15973, 2020 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-32452143

RESUMO

In situ exsolution of metal nanoparticles in perovskite under reducing atmosphere is employed to generate a highly active metal-oxide interface for CO2 electrolysis in a solid oxide electrolysis cell. Atomic-scale insight is provided into the exsolution of CoFe alloy nanoparticles in La0.4 Sr0.6 Co0.2 Fe0.7 Mo0.1 O3-δ (LSCFM) by in situ scanning transmission electron microscopy (STEM) with energy-dispersive X-ray spectroscopy and DFT calculations. The doped Mo atoms occupy B sites of LSCFM, which increases the segregation energy of Co and Fe ions at B sites and improves the structural stability of LSCFM under a reducing atmosphere. In situ STEM measurements visualized sequential exsolution of Co and Fe ions, formation of CoFe alloy nanoparticles, and reversible exsolution and dissolution of CoFe alloy nanoparticles in LSCFM. The metal-oxide interface improves CO2 adsorption and activation, showing a higher CO2 electrolysis performance than the LSCFM counterparts.

10.
ChemSusChem ; 13(23): 6290-6295, 2020 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-32459062

RESUMO

CO2 electroreduction by solid oxide electrolysis cells (SOECs) can not only attenuate the greenhouse effect, but also convert surplus electrical energy into chemical energy. The adsorption and activation of CO2 on the cathode play an important role in the SOEC performance. La0.6 Sr0.4 Co0.2 Fe0.8 O3-δ -Ce0.8 Sm0.2 O2-δ (LSCF-SDC; SDC=samarium-doped ceria) is a promising SOEC cathode. However, its electrocatalytic activity still needs to be improved. In this study, Pt/SDC interfaces are constructed by decorating Pt nanoparticles onto the SDC surface. Electrochemical measurements indicate that the polarization resistance of the SOEC is decreased from 0.308 to 0.120â€…Ω cm2 , and the current density is improved from 0.913 to 1.420 A cm-2 at 1.6 V and 800 °C. Physicochemical characterizations suggest that construction of the Pt/SDC interfaces increases the oxygen vacancy concentration on the cathode and boosts CO2 adsorption and dissociation, which leads to enhanced CO2 electroreduction performance in SOECs.

11.
Adv Mater ; 32(6): e1906193, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31894628

RESUMO

Reversible exsolution and dissolution of metal nanoparticles in perovskite has been investigated as an efficient strategy to improve CO2 electrolysis performance. However, fundamental understanding with regard to the reversible exsolution and dissolution of metal nanoparticles in perovskite is still scarce. Herein, in situ exsolution and dissolution of CoFe alloy nanoparticles in Co-doped Sr2 Fe1.5 Mo0.5 O6-δ (SFMC) revealed by in situ X-ray diffraction, scanning transmission electron microscopy, environmental scanning electron microscopy, and density functional theory calculations are reported. Under a reducing atmosphere, facile exsolution of Co promotes reduction of the Fe cation to generate CoFe alloy nanoparticles in SFMC, accompanied by structure transformation from double perovskite to layered perovskite at 800 °C. Under an oxidizing atmosphere, spherical CoFe alloy nanoparticles are first oxidized to flat CoFeOx nanosheets, and then dissolved into the bulk with structure evolution from layered perovskite back to double perovskite. Electrochemically, CO2 electrolysis performance can be retrieved during 12 redox cycles due to the regenerative ability of the CoFe alloy nanoparticles. The anchoring of the CoFe alloy nanoparticles in SFMC perovskite via reduction shows enhanced CO2 electrolysis performance and stability compared with the parent SFMC perovskite.

12.
Angew Chem Int Ed Engl ; 58(45): 16043-16046, 2019 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-31468666

RESUMO

Oxidative dehydrogenation of ethane (ODE) is limited by the facile deep oxidation and potential safety hazards. Now, electrochemical ODE reaction is incorporated into the anode of a solid oxide electrolysis cell, utilizing the oxygen species generated at anode to catalytically convert ethane. By infiltrating γ-Al2 O3 onto the surface of La0.6 Sr0.4 Co0.2 Fe0.8 O3-δ -Sm0.2 Ce0.8 O2-δ (LSCF-SDC) anode, the ethylene selectivity reaches as high as 92.5 %, while the highest ethane conversion is up to 29.1 % at 600 °C with optimized current and ethane flow rate. Density functional theory calculations and in situ X-ray photoelectron spectroscopy characterizations reveal that the Al2 O3 /LSCF interfaces effectively reduce the amount of adsorbed oxygen species, leading to improved ethylene selectivity and stability, and that the formation of Al-O-Fe alters the electronic structure of interfacial Fe center with increased density of state around Fermi level and downshift of the empty band, which enhances ethane adsorption and conversion.

13.
Adv Mater ; 31(50): e1902033, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31282069

RESUMO

High-temperature CO2 electrolysis in solid-oxide electrolysis cells (SOECs) could greatly assist in the reduction of CO2 emissions by electrochemically converting CO2 to valuable fuels through effective electrothermal activation of the stable CO bond. If powered by renewable energy resources, it could also provide an advanced energy-storage method for their intermittent output. Compared to low-temperature electrochemical CO2 reduction, CO2 electrolysis in SOECs at high temperature exhibits higher current density and energy efficiency and has thus attracted much recent attention. The history of its development and its fundamental mechanisms, cathode materials, oxygen-ion-conducting electrolyte materials, and anode materials are highlighted. Electrode, electrolyte, and electrode-electrolyte interface degradation issues are comprehensively summarized. Fuel-assisted SOECs with low-cost fuels applied to the anode to decrease the overpotential and electricity consumption are introduced. Furthermore, the challenges and prospects for future research into high-temperature CO2 electrolysis in SOECs are included.

14.
Arch Oral Biol ; 103: 55-61, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31136880

RESUMO

OBJECTIVE: The aim of this study was to investigate the effects of Candida albicans on the production of defense effector molecules by human oral mucosal epithelial cells in vitro. DESIGN: Immortalized human oral mucosal epithelial (Leuk-1) cells and C. albicans strain 5314 were cocultured at different cell-to-C. albicans ratios. The viability of Leuk-1 cells was determined by MTT and RTCA measurements. The secretory levels of multiple defense effector molecules were determined by Enzyme-linked immunosorbent assay (ELISA). RESULTS: Our results indicated that C. albicans significantly decreased the secretion of IgG, cystatin C, lactoferrin, and TGF-ß1 in a dose-dependent manner and remarkably reduced the production of IgA independent of the cell-to-C. albicans ratio. However, C. albicans clearly enhanced the secretion of IgM, galectin-3, P-selectin, granzyme B and perforin. CONCLUSION: These results suggest that C. albicans may exert a regulatory role in the defense response of oral mucosal epithelial cells by altering secretory levels of defense effector molecules.


Assuntos
Candida albicans/imunologia , Candidíase , Imunidade nas Mucosas/genética , Imunidade nas Mucosas/fisiologia , Fatores Imunológicos/genética , Técnicas de Cocultura , Células Epiteliais , Humanos , Mucosa Bucal
15.
Angew Chem Int Ed Engl ; 58(14): 4617-4621, 2019 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-30737877

RESUMO

The oxygen evolution reaction (OER) is a sluggish electrocatalytic reaction in solid oxide electrolysis cells (SOECs) at high temperatures (600-850 °C). Perovskite oxide has been widely investigated for catalyzing the OER; however, the formation of cation-enriched secondary phases at the oxide/oxide interface blocks the active sites and decreases OER performance. Herein, we show that the Au/yttria-stabilized zirconia (YSZ) interface possesses much higher OER activity than the lanthanum strontium manganite/YSZ anode. Electrochemical characterization and density functional theory calculations suggest that the Au/YSZ interface provides a favorable path for OER by triggering interfacial oxygen spillover from the YSZ to the Au surface. In situ X-ray photoelectron spectroscopy results confirm the existence of spillover oxygen on the Au surface. This study demonstrates that the Au/YSZ interface possesses excellent catalytic activity for OER at high temperatures in SOECs.

16.
Artigo em Chinês | WPRIM (Pacífico Ocidental) | ID: wpr-750796

RESUMO

Objective@#To explore the relationship between psychological factors and recurrent aphthous ulcer (RAU), oral lichen planus (OLP), and burning mouth syndrome (BMS) and to provide a reference for clinical diagnosis and treatment of the disease.@*Methods@#From July to October 2018, 50 patients with common RAU, refractory RAU, OLP and BMS were selected as the observation group, and 50 healthy participants without major systemic diseases and oral mucosal diseases matched for age and sex served as the control group. The psychological status of the subjects in each group was investigated by questionnaires, including the generalized anxiety disorder 7-item scale(GAD-7) and the patient health questionnaire-9 (PHQ-9).@*Results@#Compared with the control group, the PHQ-9 scores in the refractory RAU, common RAU, OLP and BMS groups were higher than those in the control group (P < 0.05), and the GAD-7 scores in the refractory RAU, OLP and BMS groups were higher than those in the control group (P < 0.05). In the RAU group, the GAD-7 score of intractable RAU was higher than that of common RAU (P < 0.05), and there was no significant difference in the PHQ-9 score (P > 0.05).@*Conclusion @#RAU, OLP and BMS are common psychosomatic diseases presented by patients in the Department of Oral Mucosal Diseases. Their occurrence and development are related to the psychological status of patients. A tendency toward anxiety is significantly more common among refractory RAU patients than common RAU patients.

17.
Appl Opt ; 57(10): 2577-2583, 2018 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-29714243

RESUMO

The sum-frequency generation (SFG) in potassium dihydrogen phosphate (KDP) powder with µm-grade particle size is successfully demonstrated under various experimental conditions. Two focused beams of 870 nm and 1369 nm are used for SFG excitation. SFG is observed under different excitation energies. The SFG intensity shows isotropy with different observation azimuths. The intersection angle between two excitation beams is not limited by conventional phase-matching conditions, and it owns the flexibility of a very large allowed range, e.g., it can be 0°âˆ¼100° in this work. The polarization combination of excitation beams is not limited either. Thanks to the non-toxicity, low price, and low SFG threshold properties of KDP material and the optical flexibility, this powder SFG technology is a versatile method and is expected to be applied to various situations of optical alignment, e.g., surface SFG, four-wave mixing, coherent anti-Stokes Raman spectroscopy, multi-color laser excitation, etc. The effect of potential powder SFG-assisted optical alignments is also discussed. Extension of this method to multi-beams, tight focusing beams, and plasmonic polariton devices is proposed.

18.
J Dent Sci ; 13(2): 124-130, 2018 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-30895107

RESUMO

BACKGROUND/PURPOSE: Recurrent aphthous ulceration (RAU) has an incidence of approximately 20% in general population. However, its exact cause remains unknown. Increasing evidence suggests that immunologic mechanisms may play crucial roles in the etiology of this disease. MATERIALS AND METHODS: The peripheral blood samples were obtained from 85 patients with RAU during acute phase and 87 healthy controls. The serum levels of IgG, IgA, IgM, C3 and C4 were measured by immunoturbidimetry. In addition, the serum IgE levels were measured by electro-chemiluminescence immunoassay. Furthermore, the percentages of B, T, CD4+ T, CD8+ T lymphocytes and natural killer (NK) cells in peripheral blood were determined by flow cytometry. RESULTS: Our findings showed that the serum IgG, IgA, IgE, C3 and C4 levels of RAU patients were significantly higher than those of healthy controls. The percentages of CD4+ T cells and B cells in peripheral blood of RAU patients were significantly decreased, whereas the percentages of CD8+ T cells and NK cells of RAU patients were remarkably increased. Our results indicated that the IgG level was elevated in 18 patients (21.2%) and that the IgE level was increased in 21 patients (24.7%). Our results also showed that the frequency of abnormal IgG or IgE levels were significantly correlated with that of abnormal CD8+ T cell percentage in RAU patients. CONCLUSION: The levels of both humoral and cellular immune components could be altered in RAU. The relationship between humoral and cellular immune may be potentially important immunologic aspects involved in the pathogenesis of RAU.

19.
Toxins (Basel) ; 7(12): 5212-23, 2015 Dec 02.
Artigo em Inglês | MEDLINE | ID: mdl-26633508

RESUMO

Health risk of human exposure to microcystin-leucine arginine (MC-LR) has aroused more and more attention over the past few decades. In the present study, MC-LR was orally administered to female mice at 0, 1, 10 and 40 µg/L for three and six months. We found that chronic exposure to MC-LR at environmental levels could stimulate follicle atresia and lead to decreased developmental follicles, accompanied by a reduction of gonadosomatic index (GSI). In line with the irregular gonadal hormone level and estrus cycles, subfertility of female mice was also confirmed by analyzing numbers of litters and pups. The in vitro study suggested that granulosa cells could uptake MC-LR and should be the target of the toxicant. Oxidative stress in granulose cells induced by MC-LR promoted follicle atresia and eventually leads to female subfertility.


Assuntos
Células da Granulosa/efeitos dos fármacos , Infertilidade/induzido quimicamente , Microcistinas/toxicidade , Animais , Catalase/metabolismo , Células Cultivadas , Estradiol/sangue , Feminino , Atresia Folicular , Células da Granulosa/metabolismo , Masculino , Toxinas Marinhas , Camundongos , Estresse Oxidativo/efeitos dos fármacos , Progesterona/sangue , Superóxido Dismutase/metabolismo
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